三维介孔KIT-6上高分散Ni纳米粒子用于CO甲烷化:助剂对催化性能的影响

引用本文: 曹红霞, 张军, 郭成龙, 陈经广, 任相坤. 三维介孔KIT-6上高分散Ni纳米粒子用于CO甲烷化:助剂对催化性能的影响[J]. 催化学报, 2017, 38(7): 1127-1137. doi: 10.1016/S1872-2067(17)62862-6 shu

Citation: HongXia Cao, Jun Zhang, ChengLong Guo, Jingguang G. Chen, XiangKun Ren. Highly dispersed Ni nanoparticles on 3D-mesoporous KIT-6 for CO methanation:Effect of promoter species on catalytic performance[J]. Chinese Journal of Catalysis, 2017, 38(7): 1127-1137. doi: 10.1016/S1872-2067(17)62862-6 shu

三维介孔KIT-6上高分散Ni纳米粒子用于CO甲烷化:助剂对催化性能的影响

a 中国矿业大学低碳能源研究院, 江苏徐州 221008, 中国;
b 哥伦比亚大学地球与环境工程系, 纽约 10027, 美国;
c 中国矿业大学电气与动力工程学院, 江苏徐州 221116, 中国;
d 哥伦比亚大学化学工程系, 纽约 10027, 美国
基金项目:
中央高校基本科研业务费专项资金资助（2015XKMS061）.

摘要: 作为煤制天然气的核心技术之一，CO甲烷化工艺的开发基础便是高效催化剂的研制.目前，CO甲烷化催化剂主要采用Ni作为活性组分，但如何保持其具有较高的催化活性和优异的高温稳定性，仍为当今不得不面临的棘手问题.本文以乙二醇改性的三维介孔KIT-6为载体，利用其较高的比表面积、可调孔径、独特的双螺旋三维孔道结构等特点，通过湿式浸渍法成功制备了由助剂改性的Ni基催化剂，探讨了V，Ce，La，Mn等不同助剂对Ni基催化剂CO甲烷化催化性能的影响.分别采用X射线衍射、氢气程序升温还原、氢气程序升温脱附、傅里叶变换红外光谱、透射电子显微镜、能量色散X射线光谱、激光拉曼光谱和热重分析等手段对催化剂特性进行了表征.结果显示，Ni-V/KIT-6具有最高的Ni纳米粒子分散性（26.5%）和催化还原性，产生了最多的活性位，同时，Si-O-V的形成增强了金属-载体间相互作用，并因载体的三维介孔限制效应而形成较小Ni纳米粒子，这些均有助于提升Ni基催化剂CO甲烷化的催化性能和稳定性.在常压、250-400 ℃和60000mL/（g·h）空速的实验条件下对催化剂进行了催化活性评价测试.结果表明，助剂提高了CO甲烷化低温催化活性，其中，Ni-V/KIT-6在350 ℃的条件下实现了CO的完全转化，CH₄产率也高达85%；其在常压、500 ℃和60000 mL/（g·h）空速的操作条件下所进行的稳定性测试结果还显示，Ni-V/KIT-6也具有优异的抗烧结和抗积碳能力，展示了良好的高温稳定性.因此，Ni-V/KIT-6是一种具有广阔应用前景的CO甲烷化催化剂.

关键词:

English

Highly dispersed Ni nanoparticles on 3D-mesoporous KIT-6 for CO methanation:Effect of promoter species on catalytic performance

a Low Carbon Energy Institute, China University of Mining and Technology, Xuzhou 221008, Jiangsu, China;
b Earth and Environmental Engineering Department, Columbia University, New York 10027, United States;
c School of Electrical and Power Engineering, China University of Mining and Technology, Xuzhou 221116, Jiangsu, China;
d Department of Chemical Engineering, Columbia University, New York 10027, United States
Received Date: 09 April 2017
Revised Date: 23 May 2017
Fund Project:
This work was supported by the Fundamental Research Funds for the Central Universities (2015XKMS061).

Abstract: Promoter-modified Ni-based catalysts were synthesized by an incipient-wetness impregnation method using 3D-mesoporous KIT-6 as a support modified by ethylene glycol, and evaluated for the catalytic production of synthetic natural gas (SNG) from CO methanation. Characterization results suggested that the addition of promoter species could remarkably improve the low-temperature catalytic activity for CO methanation, which was due to a large dispersion of Ni nanoparticles, an enhanced interaction between metal and support as well as a confinement effect of 3D-mesopores. Among all catalysts, Ni-V/KIT-6 possessed the best catalytic performance, which was ascribed to the largest H₂ uptake of 177.6 μmol/g and Ni dispersion of 26.5%, an intimate interaction with the support from the formation of Si-O-V linkage and an enhanced confinement effect of 3D-mesopores to effectively prevent the growth of Ni nanoparticles and carbon filaments. In consequence, Ni-V/KIT-6 displayed excellent catalytic performance as well as high catalytic stability, which can be regarded as a promising candidate for CO methanation.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

三维介孔KIT-6上高分散Ni纳米粒子用于CO甲烷化:助剂对催化性能的影响

English

Highly dispersed Ni nanoparticles on 3D-mesoporous KIT-6 for CO methanation:Effect of promoter species on catalytic performance

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

三维介孔KIT-6上高分散Ni纳米粒子用于CO甲烷化:助剂对催化性能的影响

English

Highly dispersed Ni nanoparticles on 3D-mesoporous KIT-6 for CO methanation:Effect of promoter species on catalytic performance

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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